Sintering Evolving Mn2O3–LaMnO3 Perovskite Heterointerfaces as Highly Active and Durable Catalysts for Catalytic Removal of Volatile Organic Compounds

IF 4.3 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Chi Zhang, Jinyan Xiao, Jiajian Gao, Xuan Pang, Lei Yang, Shengwei Tang, Yunfa Chen, Wenxiang Tang
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Abstract

Improving the catalyst performance for the thermal oxidation reaction faces the daunting challenge of the activity–stability trade-off. Herein, an evolved heterointerface was constructed on spherical Mn2O3 nanocatalysts to achieve exceptional stability while maintaining adequate activity by simply introducing La. The generation of the active Mn3O4–Mn2O3 heterointerfaces by La doping was experimentally observed, which further segregates to the surface during thermal aging and forms epitaxially grown heterostructured LaMnO3–Mn2O3 with Mn atoms. The former can act as highly active sites for the deep oxidation of VOCs due to the richness in oxygen vacancies and Mn4+ ions, while the latter acts as the diffusion barrier to inhibit grain growth and produce advantageous reactive electronic structures around the interface. The La-modified Mn2O3 oxide reached 90% conversion in toluene oxidation at 286 °C under the high WHSV of 240,000 mL g–1 h–1 and slightly increased to 327 °C after thermal aging at 800 °C. This work provides a versatile strategy for fabricating effective oxidation catalysts with high low-temperature activity and antisintering properties for industrial applications.

Abstract Image

烧结演化的Mn2O3-LaMnO3钙钛矿异质界面作为催化脱除挥发性有机物的高效耐用催化剂
提高热氧化反应催化剂的性能面临着活性与稳定性权衡的严峻挑战。在此,在球形Mn2O3纳米催化剂上构建了一个进化的异质界面,通过简单地引入La来获得优异的稳定性,同时保持足够的活性。实验观察到La掺杂产生了活性的Mn3O4-Mn2O3异质界面,在热时效过程中,这些异质界面进一步向表面偏析,形成具有Mn原子的外延生长的异质结构LaMnO3-Mn2O3。前者由于丰富的氧空位和Mn4+离子,可以作为VOCs深度氧化的高活性位点,而后者则作为扩散屏障,抑制晶粒生长,并在界面周围产生有利的反应性电子结构。在24万mL g-1 h-1的高WHSV下,la改性的Mn2O3氧化物在286℃甲苯氧化中转化率达到90%,在800℃热老化后转化率略微提高到327℃。这项工作为工业应用中制造具有高低温活性和抗烧结性能的有效氧化催化剂提供了一种通用策略。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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